We investigated the Rydberg-state excitation process of a hydrogen atom subjected to spatially homogeneous and inhomogeneous laser fields by means of ab initio calculations. It is found that, comparing with atoms exposed to spatially homogeneous laser fields, the excitation probability decreases and the electron tends to occupy the states with lower principal quantum numbers and angular quantum numbers for atoms in spatially inhomogeneous laser pulses. Furthermore, calculations of a quantum model without taking into account ionization of the electron after it is coherently captured by the Rydberg state are inconsistent with the above-stated findings by ab initio calculations. Analysis indicates that the aforementioned intriguing features can be attributed to the enhanced ionization of the Rydberg states by inhomogeneous laser fields since the distributions of Rydberg states of high principal quantum numbers and angular quantum numbers locate far away from the core where the inhomogeneous electric fields become significant.
We investigated the Rydberg-state excitation process of a hydrogen atom subjected to spatially homogeneous and inhomogeneous laser fields by means of ab initio calculations. It is found that, comparing with atoms exposed to spatially homogeneous laser fields, the excitation probability decreases and the electron tends to occupy the states with lower principal quantum numbers and angular quantum numbers for atoms in spatially inhomogeneous laser pulses. Furthermore, calculations of a quantum model without taking into account ionization of the electron after it is coherently captured by the Rydberg state are inconsistent with the above-stated findings by ab initio calculations. Analysis indicates that the aforementioned intriguing features can be attributed to the enhanced ionization of the Rydberg states by inhomogeneous laser fields since the distributions of Rydberg states of high principal quantum numbers and angular quantum numbers locate far away from the core where the inhomogeneous electric fields become significant.
The dynamics of hydrogen atom in the presence of a strong radiation field of the titanium-sapphire laser is studied for the Keldysh parameters γ ≥ 1 and γ ≤ 1. It is demonstrated that the ionization is supplemented with the effective population of the excited states with the principal quantum numbers n = 5–10 in the entire range of variation in the Keldysh parameter. The population of the excited Rydberg states can be interpreted as a consequence of the multiphoton resonance involving the initial 1 s state and a group of excited states in the vicinity of the continuum boundary with the simultaneous repopulation of these states by Λ-type Raman transitions under the action of the laser field. The resulting coherent Rydberg packet appears to be stable with respect to ionization, so that the ionization of the atomic system in the presence of strong electromagnetic field is suppressed. Physical reasons for the stabilization are discussed. An interpretation of the effective population of the Rydberg states in the recent experiments on the ionization of atomic helium by the titanium-sapphire laser is proposed.
An extension of the model of Merkt and Zare [J. Chem. Phys. 101, 3495 (1994)] is presented to describe the effects of static inhomogeneous electric fields, which arise experimentally from combinations of applied (or stray) homogeneous fields and the presence of charged particles, on Rydberg states of atoms and molecules. The effect of an arbitrary number of charged particles is included and the effects of nonzero quantum defects are investigated. A quantization axis rotation procedure is defined, allowing clear distinction between homogeneous and inhomogeneous field effects. Calculations are reported of the time-dependent decay of a coherent population of eigenstates for n=20, 33, and 50, involving diagonalization of the full n2×n2 matrix. Calculations are also carried out for n=100 by pre-diagonalization of the full homogeneous field perturbation followed by a restricted basis set diagonalization for the inhomogeneous part of the perturbation. The inclusion of nonzero quantum defects has a substantial impact on the ml mixing, confining significant mixing to a narrow range of radial and angular positions of the ion. An applied homogeneous field of order the Inglis-Teller field is required in combination with the field due to the ions. The dynamics are very different according to whether np or nf series carry the transition probability. For np-state population, the maximum stabilization is achieved at ion-Rydberg distances of around 5n2a0, with the ion almost perpendicular to the applied homogeneous field. For an initial nf population the ion perturbation may have a destabilizing effect at sufficiently small homogeneous field (⩽0.1FIT). Significant effects of laser polarization on the stability are reported. Calculations for a realistic pseudo-random distribution of ions and Rydbergs suggest that ml mixing by ions will never reach the complete mixing limit, but that at least an order of magnitude stabilization is achievable under a restricted range of conditions.
Using field ionization combined with the direct detection of excited neutral atoms we measured the distribution of principal quantum number n of excited He Rydberg states after strong-field excitation at laser intensities well in the tunneling regime. Our results confirm theoretical predictions from semiclassical and quantum mechanical calculations and simultaneously underpin the validity of the semiclassical frustrated tunneling ionization model. Moreover, since our experimental detection scheme is spin sensitive in the case of He atoms, we show that strong-field excitation leads to strong population of triplet states. The origin of it lies in the fact that high angular momentum states are accessible in strong-field excitation. Thus, singlet-triplet transitions become possible due to the increased importance of spin-orbit interaction rather than due to direct laser induced spin-flip processes.
The outer electron of a Rydberg atom is so weakly bound to the atomic core that a relatively small electric field may cause the electron to be stripped from the atom. The field strength at which this ionization happens is strongly dependent on the state of the Rydberg atom. Pulsed electric field ionization serves, therefore, not only as a means by which a Rydberg atom may be efficiently detected, but also a means by which the state of the Rydberg atom may be analyzed.\nThe first observation of predominantly diabatic passage to field ionization of a non-hydrogenic Rydberg atom has resulted in an improved understanding of the adiabatic and diabatic ionization processes. The magnitudes of the various field ionization features have been measured and found to agree with theory, and by detailed analysis, it is now possible to label the various field ionization signal features with the appropriate (VBAR)m(,l)(VBAR) quantum numbers. A much better understanding of the laser excitation process, the Rydberg state production, and the response of the excited state to an increasing electric field has enabled measurement of some Rydberg fine-structure intervals, through observation of field ionization quantum beats.
Rather than being freed to the continuum, the strong-field tunneled electrons can make a trajectory driven by the remaining laser fields and have certain probability to be captured by the high lying Rydberg states of the parent atoms or molecules. To explore the effect of molecular orbital on Rydberg state excitation, the ellipticity dependence of Rydberg state yields of N2 and O2 molecules are experimentally investigated using cold target recoil ion momentum spectroscopy and are compared with their counterpart atoms Ar and Xe with comparable ionization potentials. We found the generation probability of the neutral Rydberg fragment O2* was orders of magnitude higher than that of Xe* due to the butterfly-shaped highest occupied molecular orbital of O2. Meanwhile, our experimental and simulation results reveal that it is the initial momentum distribution (determined by the detailed characteristics of orbitals) that finally leads to the tendency that the Rydberg state yield of O2 (Ar) decreased slower than that obtained for Xe (N2) when the ellipticity of the excitation laser field is increased.
High-order harmonic spectra and attosecond pulse generation from Rydberg atom (He[Formula: see text]) driven by the spatially inhomogeneous field have been theoretically investigated. (i) Firstly, with an electron initially in a single excited Rydberg state (nth), the harmonic yield can be enhanced due to the decreased ionization potential, and a maximum enhancement can be obtained when the initial state is prepared as the third excited state (n = 3). However, the low cutoff energy from the excited state is unbeneficial to the generation of the higher photon pulse. Thus, with the further introduction of the laser chirp, not only the harmonic cutoff is extended, but also the harmonic modulation is reduced. As a result, five super-bandwidths from 63 eV to 267 eV can be found. (ii) Secondly, by preparing the initial state as a coherent superposition of excited state, the harmonic yield can be further enhanced, especially for the coherent superposition of the first and the third (n = 1 + 3) and the second and the fourth (n = 2 + 4) excited states, the harmonic yield is enhanced by 4–8 orders of magnitude compared with the case of the single ground initial state. Furthermore, by properly adding the laser pulse into the spatially inhomogeneous region (gap center [Formula: see text] a.u.) from left [Formula: see text] to right [Formula: see text], much higher cutoff energies can be obtained in the left region. As a consequence, two super-bandwidths of 248 eV and 496 eV can be obtained. Finally, by properly superposing the harmonics, a series of sub-25-as pulses with intensity enhancement of 5–8 orders of magnitude can be produced.